Solar-to-chemical energy conversion schemes are of interest in the pursuit of renewable energy sources. One attractive approach is the photocatalytic reduction of protons to hydrogen fuel via homogeneous catalysis whereby photoexcitation of a light absorber generates high-energy species that must undergo multiple structural and electronic modifications prior to catalysis. The ability to use low energy light to initiate catalysis would be beneficial given the relatively high solar power density of visible light that reaches the Earth’s surface. Our current research involves the use of formamidinate-bridged Rh2II,II dimers of the design [Rh2II,II(μ-form)2(NN)2](BF4)2 (μ-form = formamidinate bridge; NN = diimine ligand) as visible light absorbers and potential single-component photocatalysts. The electrochemical and photophysical properties are impacted by the mode of diimine ligand coordination (κ2-NN bidentate and µ2-NN bridging) and assist in the design of potentially active photocatalysts for H2 production. Transient absorption spectroscopy, TD-DFT calculations, and electrochemistry have been utilized to provide insight into populated excited states and deactivation processes that occur after low energy photoexcitation.

Monitoring the excited state properties of dirhodium(II,II) complexes following visible light photoexcitation with potential applications in solar energy conversion

251st National Meeting (2016)

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